电合成高附加值多元碳化合物与制氢相结合是实现碳中和的有效途径;然而,电合成中缺乏有效的双功能催化剂在很大程度上阻碍了其发展。
本文报道了以1nm PtIr纳米线(NWs)为双功能催化剂,在阳极和阴极分别高效电合成高附加值的1,1-二乙氧基乙烷(DEE)和高纯氢的第一个实例。研究人员发现,使用1nm PtIr纳米线作为双功能催化剂的电池可以达到0.61V的最低电压,达到10mA cm–2的电流密度,远低于Pt NWs(0.85V)和商用Pt/C(0.86V)的电流密度。在所有报道的电合成催化剂中,DEE和析氢的法拉第效率最高,分别为85%和94.0%。
原位红外光谱研究表明,PtIr-NWs能促进乙醇中O-H和C-H键的活化,这对乙醛中间体的形成和最终DEE的合成具有重要意义。此外,以PtIr-NWs为双功能催化剂的电池显示出良好的稳定性,几乎没有明显降低DEE产品的法拉第效率。
附:英文原文
Title: One Nanometer PtIr Nanowires as High-Efficiency Bifunctional Catalysts for Electrosynthesis of Ethanol into High Value-Added Multicarbon Compound Coupled with Hydrogen Production
Author: Kun Yin, Yuguang Chao, Fan Lv, Lu Tao, Weiyu Zhang, Shiyu Lu, Menggang Li, Qinghua Zhang, Lin Gu, Hongbo Li, Shaojun Guo
Issue&Volume: July 19, 2021
Abstract: The electrosynthesis of high-value-added multicarbon compounds coupled with hydrogen production is an efficient way to achieve carbon neutrality; however, the lack of effective bifunctional catalysts in electrosynthesis largely hinders its development. Herein, we report the first example on the highly efficient electrosynthesis of high-value-added 1,1-diethoxyethane (DEE) at the anode and high-purity hydrogen at the cathode using 1 nm PtIr nanowires (NWs) as the bifunctional catalysts. We demonstrate that the cell using 1 nm PtIr nanowires as the bifunctional catalysts can achieve a reported lowest voltage of 0.61 V to reach the current density of 10 mA cm–2, much lower than those of the Pt NWs (0.85 V) and commercial Pt/C (0.86 V), and also can have the highest Faraday efficiencies of 85% for DEE production and 94.0% for hydrogen evolution in all the reported electrosynthesis catalysts. The in situ infrared spectroscopy study reveals that PtIr NWs can facilitate the activation of O–H and C–H bonds in ethanol, which is important for the formation of acetaldehyde intermediate, and finally DEE. In addition, the cell using PtIr NWs as bifunctional catalysts exhibits excellent stability by showing almost no obvious decrease in the Faraday efficiency of the DEE production.
DOI: 10.1021/jacs.1c04626
Source: https://pubs.acs.org/doi/10.1021/jacs.1c04626
JACS:《美国化学会志》,创刊于1879年。隶属于美国化学会,最新IF:14.612
官方网址:https://pubs.acs.org/journal/jacsat
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